Photo-Assisted Ferroelectric Domain Control for α-In2Se3 Artificial Synapses Inspired by Spontaneous Internal Electric Fields.

α-In2Se3 semiconductor crystals realize artificial synapses by tuning in-plane and out-of-plane ferroelectricity with diverse avenues of electrical and optical pulses. While the electrically induced ferroelectricity of α-In2Se3 shows synaptic memory operation, the optically assisted synaptic plasticity in α-In2Se3 has also been preferred for polarization flipping enhancement. Here, the synaptic memory behavior of α-In2Se3 is demonstrated by applying electrical gate voltages under white light. As a result, the induced internal electric field is identified at a polarization flipped conductance channel in α-In2Se3/hexagonal boron nitride (hBN) heterostructure ferroelectric field effect transistors (FeFETs) under white light and discuss the contribution of this built-in electric field on synapse characterization. The biased dipoles in α-In2Se3 toward potentiation polarization direction by an enhanced internal built-in electric field under illumination of white light lead to improvement of linearity for long-term depression curves with proper electric spikes. Consequently, upon applying appropriate electric spikes to α-In2Se3/hBN FeFETs with illuminating white light, the recognition accuracy values significantly through the artificial learning simulation is elevated for discriminating hand-written digit number images.

Reliable synaptic plasticity of InGaZnO transistor with TiO2interlayer.

We demonstrate an InGaZnO (IGZO)-based synaptic transistor with a TiO2buffer layer. The structure of the synaptic transistor with TiO2inserted between the Ti metal electrode and an IGZO semiconductor channel O2trapping layer produces a large hysteresis window, which is crucial for achieving synaptic functionality. The Ti/TiO2/IGZO synaptic transistor exhibits reliable synaptic plasticity features such as excitatory post-synaptic current, paired-pulse facilitation, and potentiation and depression, originating from the reversible charge trapping and detrapping in the TiO2layer. Finally, the pattern recognition accuracy of Modified National Institute of Standards and Technology handwritten digit images was modeled using CrossSim simulation software. The simulation results present a high image recognition accuracy of ∼89%. Therefore, this simple approach using an oxide buffer layer can aid the implementation of high-performance synaptic devices for neuromorphic computing systems.

Increased Mobility and Reduced Hysteresis of MoS2 Field-Effect Transistors via Direct Surface Precipitation of CsPbBr3-Nanoclusters for Charge Transfer Doping.

Transition-metal dichalcogenides (TMDs) and metal halide perovskites (MHPs) have been investigated for various applications, owing to their unique physical properties and excellent optoelectronic functionalities. TMD monolayers synthesized via chemical vapor deposition (CVD), which are advantageous for large-area synthesis, exhibit low mobility and prominent hysteresis in the electrical signals of field-effect transistors (FETs) because of their native defects. In this study, we demonstrate an increase in electrical mobility by ∼170 times and reduced hysteresis in the current-bias curves of MoS2 FETs hybridized with CsPbBr3 for charge transfer doping, which is implemented via solution-based CsPbBr3-nanocluster precipitation on CVD-grown MoS2 monolayer FETs. Electrons injected from CsPbBr3 into MoS2 induce heavy n-doping and heal point defects in the MoS2 channel layer, thus significantly increasing mobility and reducing hysteresis in the hybrid FETs. Our results provide a foundation for improving the reliability and performance of TMD-based FETs by hybridizing them with solution-based perovskites.

Reinforcing Synaptic Plasticity of Defect-Tolerant States in Alloyed 2D Artificial Transistors.

While two-dimensional (2D) materials possess the desirable future of neuromorphic computing platforms, unstable charging and de-trapping processes, which are inherited from uncontrollable states, such as the interface trap between nanocrystals and dielectric layers, can deteriorate the synaptic plasticity in field-effect transistors. Here, we report a facile and effective strategy to promote artificial synaptic devices by providing physical doping in 2D transition-metal dichalcogenide nanomaterials. Our experiments demonstrate that the introduction of niobium (Nb) into 2D WSe2 nanomaterials produces charge trap levels in the band gap and retards the decay of the trapped charges, thereby accelerating the artificial synaptic plasticity by encouraging improved short-/long-term plasticity, increased multilevel states, lower power consumption, and better symmetry and asymmetry ratios. Density functional theory calculations also proved that the addition of Nb to 2D WSe2 generates defect tolerance levels, thereby governing the charging and de-trapping mechanisms of the synaptic devices. Physically doped electronic synapses are expected to be a promising strategy for the development of bioinspired artificial electronic devices.

Conduction Mechanism in Acceptor- or Donor-Doped ZrO2 Bulk and Thin Films.

The leakage current in capacitors in future electronics should be highly suppressed to achieve low power consumption, high reliability, and fast data processing. Although considerable efforts have been directed at reducing the leakage current, fundamental studies on the effects of doping on bulk and thin-film materials have rarely been conducted. Herein, we investigated the effects of doping with acceptor and donor elements on the conduction of bulk and thin-film ZrO2 and elucidated the underlying charge conduction mechanism. In the case of bulk ZrO2, the electrical conductivity was reliably modulated by the type of dopant element, which is highly consistent with defect chemistry theory. However, unlike in the bulk material, in acceptor- and donor-doped thin-film ZrO2, the leakage current was suppressed, indicating that the factors determining the electrical property in thin films are different from those in bulk materials.

Robust 2D MoS2 Artificial Synapse Device Based on a Lithium Silicate Solid Electrolyte for High-Precision Analogue Neuromorphic Computing.

High-precision artificial synaptic devices compatible with existing CMOS technology are essential for realizing robust neuromorphic hardware systems with reliable parallel analogue computation beyond the von Neumann serial digital computing architecture. However, critical issues related to reliability and variability, such as nonlinearity and asymmetric weight updates, have been great challenges in the implementation of artificial synaptic devices in practical neuromorphic hardware systems. Herein, a robust three-terminal two-dimensional (2D) MoS2 artificial synaptic device combined with a lithium silicate (LSO) solid-state electrolyte thin film is proposed. The rationally designed synaptic device exhibits excellent linearity and symmetry upon electrical potentiation and depression, benefiting from the reversible intercalation of Li ions into the MoS2 channel. In particular, extremely low cycle-to-cycle variations (3.01%) during long-term potentiation and depression processes over 500 pulses are achieved, causing statistical analogue discrete states. Thus, a high classification accuracy of 96.77% (close to the software baseline of 98%) is demonstrated in the Modified National Institute of Standards and Technology (MNIST) simulations. These results provide a future perspective for robust synaptic device architecture of lithium solid-state electrolytes stacked with 2D van der Waals layered channels for high-precision analogue neuromorphic computing systems.

Highly Reproducible Heterosynaptic Plasticity Enabled by MoS2/ZrO2-x Heterostructure Memtransistor.

Electrically tunable resistive switching of a polycrystalline MoS2-based memtransistor has attracted a great deal of attention as an essential synaptic component of neuromorphic circuitry because its switching characteristics from the field-induced migration of sulfur defects in the MoS2 grain boundaries can realize multilevel conductance tunability and heterosynaptic functionality. However, reproducible switching properties in the memtransistor are usually disturbed by the considerable difficulty in controlling the concentration and distribution of the intrinsically existing sulfur defects. Herein, we demonstrate reliable heterosynaptic characteristics using a memtransistor device with a MoS2/ZrO2-x heterostructure. Compared to the control device with the MoS2 semiconducting channel, the Schottky barrier height was more effectively modulated by the insertion of the insulating ZrO2-x layer below the MoS2, confirmed by an ultraviolet photoelectron spectroscopy analysis and the corresponding energy-band structures. The MoS2/ZrO2-x memtransistor accomplishes dual-terminal (drain and gate electrode) stimulated multilevel conductance owing to the tunable resistive switching behavior under varying gate voltages. Furthermore, the memtransistor exhibits long-term potentiation/depression endurance cycling over 7000 pulses and stable pulse cycling behavior by the pulse stimulus from different terminal regions. The promising candidate as an essential synaptic component of the MoS2/ZrO2-x memtransistors for neuromorphic systems results from the high recognition accuracy (∼92%) of the deep neural network simulation test, based on the training and inference of handwritten numbers (0-9). The simple memtransistor structure facilitates the implementation of complex neural circuitry.

In-depth analysis on electrical parameters of floating gate IGZO synaptic transistor affecting pattern recognition accuracy.

The reliable conductance modulation of synaptic devices is key when implementing high-performance neuromorphic systems. Herein, we propose a floating gate indium gallium zinc oxide (IGZO) synaptic device with an aluminum trapping layer to investigate the correlation between its diverse electrical parameters and pattern recognition accuracy. Basic synaptic properties such as excitatory postsynaptic current, paired pulse facilitation, long/short term memory, and long-term potentiation/depression are demonstrated in the IGZO synaptic transistor. The effects of pulse tuning conditions associated with the pulse voltage magnitude, interval, duration, and cycling number of the applied pulses on the conductance update are systematically investigated. It is discovered that both the nonlinearity of the conductance update and cycle-to-cycle variation should be critically considered using an artificial neural network simulator to ensure the high pattern recognition accuracy of Modified National Institute of Standards and Technology (MNIST) handwritten digit images. The highest recognition rate of the MNIST handwritten dataset is 94.06% for the most optimized pulse condition. Finally, a systematic study regarding the synaptic parameters must be performed to optimize the developed synapse device.

In-depth analysis on electrical parameters of floating gate IGZO synaptic transistor affecting pattern recognition accuracy.

The reliable conductance modulation of synaptic devices is key when implementing high-performance neuromorphic systems. Herein, we propose a floating gate IGZO synaptic device with an aluminum trapping layer to investigate the correlation between its diverse electrical parameters and pattern recognition accuracy. Basic synaptic properties such as excitatory postsynaptic current, paired pulse facilitation, long/short term memory, and long-term potentiation/depression are demonstrated in the IGZO synaptic transistor. The effects of pulse tuning conditions associated with the pulse voltage magnitude, interval, duration, and cycling number of the applied pulses on the conductance update are systematically investigated. It is discovered that both the nonlinearity of the conductance update and cycle-to-cycle variation should be critically considered using an artificial neural network simulator to ensure the high pattern recognition accuracy of Modified National Institute of Standards and Technology (MNIST) handwritten digit images. The highest recognition rate of the MNIST handwritten dataset is 94.06% for the most optimized pulse condition. Finally, a systematic study regarding the synaptic parameters must be performed to optimize the developed synapse device.

Accelerated Learning in Wide-Band-Gap AlN Artificial Photonic Synaptic Devices: Impact on Suppressed Shallow Trap Level.

Artificial synaptic platforms are promising for next-generation semiconductor computing devices; however, state-of-the-art optoelectronic approaches remain challenging, owing to their unstable charge trap states and limited integration. We demonstrate wide-band-gap (WBG) III-V materials for photoelectronic neural networks. Our experimental analysis shows that the enhanced crystallinity of WBG synapses promotes better synaptic characteristics, such as effective multilevel states, a wider dynamic range, and linearity, allowing the better power consumption, training, and recognition accuracy of artificial neural networks. Furthermore, light-frequency-dependent memory characteristics suggest that artificial optoelectronic synapses with improved crystallinity support the transition from short-term potentiation to long-term potentiation, implying a clear emulation of the psychological multistorage model. This is attributed to the charge trapping in deep-level states and suppresses fast decay and nonradiative recombination in shallow traps. We believe that the fingerprints of these WBG synaptic characteristics provide an effective strategy for establishing an artificial optoelectronic synaptic architecture for innovative neuromorphic computing.

Ultra-flexible and rollable 2D-MoS2/Si heterojunction-based near-infrared photodetector via direct synthesis.

Atomic two-dimensional (2D) transition metal dichalcogenides (TMDs) have attracted significant attention for application in various optoelectronic devices such as image sensors, biomedical imaging systems, and consumer electronics and in diverse spectroscopic analyses. However, a complicated fabrication process, involving transfer and alignment of as-synthesized 2D layers onto flexible target substrates, hinders the development of flexible high-performance heterojunction-based photodetectors. Herein, an ultra-flexible 2D-MoS2/Si heterojunction-based photodetector is successfully fabricated through atmospheric-pressure plasma enhanced chemical vapor deposition, which enables the direct deposition of multi-layered MoS2 onto a flexible Si substrate at low temperature (<200 °C). The photodetector is responsive to near infrared light (λ = 850 nm), showing responsivity of 10.07 mA W-1 and specific detectivity (D*) of 4.53 × 1010 Jones. The measured photocurrent as a function of light intensity exhibits good linearity with a power law exponent of 0.84, indicating negligible trapping/de-trapping of photo-generated carriers at the heterojunction interface, which facilitates photocarrier collection. Furthermore, the photodetectors can be bent with a small bending radius (5 mm) and wrapped around a glass rod, showing excellent photoresponsivity under various bending radii. Hence, the device exhibits excellent flexibility, rollability, and durability under harsh bending conditions. This photodetector has significant potential for use in next-generation flexible and patchable optoelectronic devices.

Novel Exfoliation of High-Quality 2H-MoS2 Nanoflakes for Solution-Processed Photodetector.

Highly dispersive molybdenum disulfide nanoflakes (MoS2 NFs), without any phase transition during the exfoliation process, are desirable for full utilization of their semiconductor properties in practical applications. Here, we demonstrate an innovate approach for fabricating MoS2 NFs by using hydrazine-assisted ball milling via the synergetic effect of chemical intercalation and mechanical exfoliation. The NFs obtained have a lateral size of 600-800 nm, a thickness less than 3 nm, and high crystallinity in the 2H semiconducting phase. They form a stable dispersion in various solvents, which will be helpful for many applications, due to the oxygen functional group. To investigate production of a two-dimensional (2D) photodetector, 2D semiconducting MoS2, MoS2-p-Si vertical devices were fabricated, and their optical properties were characterized. The photodiode exhibited consistent responses with excellent photo-switching characteristics with wavelengths of 850, 530, and 400 nm.

Preparation and Properties of 2D Materials.

Since the great success of graphene, atomically thin layered nanomaterials-called two-dimensional (2D) materials-have attracted tremendous attention due to their extraordinary physical properties [...].

One-step H2S reactive sputtering for 2D MoS2/Si heterojunction photodetector.

A technique for directly growing two-dimensional (2D) materials onto conventional semiconductor substrates, enabling high-throughput and large-area capability, is required to realise competitive 2D transition metal dichalcogenide devices. A reactive sputtering method based on H2S gas molecules and sequential in situ post-annealing treatment in the same chamber was proposed to compensate for the relatively deficient sulfur atoms in the sputtering of MoS2 and then applied to a 2D MoS2/p-Si heterojunction photodevice. X-ray photoelectron, Raman, and UV-visible spectroscopy analysis of the as-deposited Ar/H2S MoS2 film were performed, indicating that the stoichiometry and quality of the as-deposited MoS2 can be further improved compared with the Ar-only MoS2 sputtering method. For example, Ar/H2S MoS2 photodiode has lower defect densities than that of Ar MoS2. We also determined that the factors affecting photodetector performance can be optimised in the 8-12 nm deposited thickness range.

Artificial 2D van der Waals Synapse Devices via Interfacial Engineering for Neuromorphic Systems.

Despite extensive investigations of a wide variety of artificial synapse devices aimed at realizing a neuromorphic hardware system, the identification of a physical parameter that modulates synaptic plasticity is still required. In this context, a novel two-dimensional architecture consisting of a NbSe2/WSe2/Nb2O5 heterostructure placed on an SiO2/p+ Si substrate was designed to overcome the limitations of the conventional silicon-based complementary metal-oxide semiconductor technology. NbSe2, WSe2, and Nb2O5 were used as the metal electrode, active channel, and conductance-modulating layer, respectively. Interestingly, it was found that the post-synaptic current was successfully modulated by the thickness of the interlayer Nb2O5, with a thicker interlayer inducing a higher synapse spike current and a stronger interaction in the sequential pulse mode. Introduction of the Nb2O5 interlayer can facilitate the realization of reliable and controllable synaptic devices for brain-inspired integrated neuromorphic systems.

Improvement of the Bias Stress Stability in 2D MoS2 and WS2 Transistors with a TiO2 Interfacial Layer.

The fermi-level pinning phenomenon, which occurs at the metal-semiconductor interface, not only obstructs the achievement of high-performance field effect transistors (FETs) but also results in poor long-term stability. This paper reports on the improvement in gate-bias stress stability in two-dimensional (2D) transition metal dichalcogenide (TMD) FETs with a titanium dioxide (TiO2) interfacial layer inserted between the 2D TMDs (MoS2 or WS2) and metal electrodes. Compared to the control MoS2, the device without the TiO2 layer, the TiO2 interfacial layer deposited on 2D TMDs could lead to more effective carrier modulation by simply changing the contact metal, thereby improving the performance of the Schottky-barrier-modulated FET device. The TiO2 layer could also suppress the Fermi-level pinning phenomenon usually fixed to the metal-semiconductor interface, resulting in an improvement in transistor performance. Especially, the introduction of the TiO2 layer contributed to achieving stable device performance. Threshold voltage variation of MoS2 and WS2 FETs with the TiO2 interfacial layer was ~2 V and ~3.6 V, respectively. The theoretical result of the density function theory validated that mid-gap energy states created within the bandgap of 2D MoS2 can cause a doping effect. The simple approach of introducing a thin interfacial oxide layer offers a promising way toward the implementation of high-performance 2D TMD-based logic circuits.

Improved electrical performance of a sol-gel IGZO transistor with high-k Al2O3 gate dielectric achieved by post annealing.

We have explored the effect of post-annealing on the electrical properties of an indium gallium zinc oxide (IGZO) transistor with an Al2O3 bottom gate dielectric, formed by a sol-gel process. The post-annealed IGZO device demonstrated improved electrical performance in terms of threshold variation, on/off ratio, subthreshold swing, and mobility compared to the non-annealed reference device. Capacitance-voltage measurement confirmed that annealing can lead to enhanced capacitance properties due to reduced charge trapping. Depth profile analysis using X-ray photoelectron spectroscopy proved that percentage of both the oxygen vacancy (VO) and the hydroxyl groups (M-OH) within the IGZO/Al2O3 layers, which serve as a charge trapping source, can be substantially reduced by annealing the fabricated transistor device. Furthermore, the undesired degradation of the contact interface between source/drain electrode and the channel, which mainly concerns VO, can be largely prevented by post-annealing. Thus, the facile annealing process also improves the electrical bias stress stability. This simple post annealing approach provides a strategy for realising better performance and reliability of the solid sol-gel oxide transistor.

Facile fabrication of ZnO nanowire memory device based on chemically-treated surface defects.

In this study, we demonstrate a transistor-type ZnO nanowire (NW) memory device based on the surface defect states of a rough ZnO NW, which is obtained by introducing facile H2O2 solution treatment. The surface defect states of the ZnO NW are validated by photoluminescence characterisation. A memory device based on the rough ZnO NW exhibits clearly separated bi-stable states (ON and OFF states). A significant current fluctuation does not exist during repetitive endurance cycling test. Stable memory retention characteristics are also achieved at a high temperature of 85 °C and at room temperature. The surface-treated ZnO NW device also exhibits dynamically well-responsive pulse switching under a sequential pulse test configuration, thereby indicating its potential practical memory applications. The simple chemical treatment strategy can be widely used for modulating the surface states of diverse low-dimensional materials.

In-depth Investigation of Hg2Br2 Crystal Growth and Evolution.

Physical vapor transport (PVT) has frequently been adopted for the synthesis of mercurous bromide (Hg2Br2) single crystals for acousto-optic modulators. However, thus far, very few in-depth studies have been conducted that elucidate the growth process of the Hg2Br2 single crystal. This paper reports an in-depth investigation regarding the crystal growth and evolution behavior of the Hg2Br2 crystal with facet growth mode. Based on the experimental and simulation results, the temperature profile conditions concerning the seed generation and seed growth could be optimized. Next, the PVT-grown Hg2Br2 crystals (divided into single crystal and quasi-single crystal regions) were characterized using various analysis techniques. The single-crystal Hg2Br2 was found to possess a more uniform strain than that of the quasi-single crystal through a comparison of the X-ray diffraction data. Meanwhile, the binding energy states and electron backscatter diffraction images of the as-synthesized Hg2Br2 crystals were similar, regardless of the crystal type. Furthermore, Raman spectroscopy and transmission electron microscopy analyses provided information on the atomic vibration mode and atomic structures of the two kinds of samples. The synergistic combination of the simulation and experimental results used to verify the growth mechanism facilitates the synthesis of high-quality Hg2Br2 crystals for potential acousto-optic tunable filter device applications.

Facile Fabrication of a Two-Dimensional TMD/Si Heterojunction Photodiode by Atmospheric-Pressure Plasma-Enhanced Chemical Vapor Deposition.

A growth technique to directly prepare two-dimensional (2D) materials onto conventional semiconductor substrates, enabling low-temperature, high-throughput, and large-area capability, is needed to realize competitive 2D transition-metal dichalcogenide (TMD)/three-dimensional (3D) semiconductor heterojunction devices. Therefore, we herein successfully developed an atmospheric-pressure plasma-enhanced chemical vapor deposition (AP-PECVD) technique, which could grow MoS2 and WS2 multilayers directly onto PET flexible substrate as well as 4-in. Si substrates at temperatures of <200 °C. The as-fabricated MoS2/Si and WS2/Si heterojunctions exhibited large and fast photocurrent responses under illumination of a green light. The measured photocurrent was linearly proportional to the laser power, indicating that trapping and detrapping of the photogenerated carriers at defect states could not significantly suppress the collection of photocarriers. All the results demonstrated that our AP-PECVD method could produce high-quality TMD/Si 2D-3D heterojunctions for optoelectronic applications.